Electrical control of single-photon emission in highly-charged individual colloidal quantum dots
Sergii Morozov, Evangelina L. Pensa, Ali Hossain Khan, Anatolii Polovitsyn, Emiliano Cortes, Stefan A. Maier, Stefano Vezzoli, Iwan Moreels, Riccardo Sapienza
Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single quantum dot LEDs. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than twelve electrons and one hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot photodynamics, with an observed 210-fold increase of the decay rate, accompanied by 12-fold decrease of the emission intensity, while preserving single-photon emission characteristics. These results pave the way for deterministic control over the charge state, and room-temperature decay-rate engineering for colloidal quantum dot-based classical and quantum communication technologies.
The lattice mismatch strain field of core/multishell structures with spherical symmetry is modeled by a linear continuum elasticity approach. The effect of the strain on the energy structure and linear optical absorption in large core/shell/shell spherical semiconductor quantum dots is analyzed. Localization of the photoexcited carriers induced by coating is found to play an important role in explaining the optical stability of large CdSe/CdS/ZnS and ZnTe/ZnSe/ZnS quantum dots.
Colloidal quantum dots have garnered active research interest as quantum emitters due to their robust synthesis process and straightforward integration with nanophotonic platforms. However, obtaining indistinguishable photons from the colloidal quantum dots at room temperature is fundamentally challenging because they suffer from an extremely large dephasing rate. Here we propose an experimentally feasible method of obtaining indistinguishable single photons from an incoherently pumped solution-processed colloidal quantum dot coupled to a system of nanocavities. We show that by coupling a coll…
The coupling between single photon emitters and integrated photonic circuits is an emerging topic relevant for quantum information science and other nanophotonic applications. We investigate the coupling between a hybrid system of colloidal quantum dots and propagating gap modes of a silicon nitride waveguide system. We furthermore explore the density of optical states of the system by using a scanning probe technique and find that the quantum dots couple significantly to the photonic circuit. Our results indicate that a scalable slot-waveguide might serve as a promising platform in future dev…
Quantum dots play a promising role in the development of novel optical and biosensing devices. In this study, we investigated steady-state and time-dependent luminescence properties of InGaP/ZnS core/shell colloidal quantum dots in a solution phase at room temperature. The steady state experiments exhibited an emission maximum at 650 nm with full width at half maximum of ~ 85 nm, and strong first-excitonic absorption peak at 600 nm. The time-resolved luminescence measurements depicted a bi-exponential decay profile with lifetimes of τ1\sim 47 ns and τ 2\sim 142 ns at the emission maximum. Addi…
Solution processible colloidal quantum dots hold great promise for realizing single-photon sources embedded into scalable quantum technology platforms. However, the high-yield integration of large numbers of individually addressable colloidal quantum dots in a photonic circuit has remained an outstanding challenge. Here, we report on integrating individual colloidal core-shell quantum dots (CQDs) into a nanophotonic network that allows for excitation and efficient collection of single-photons via separate waveguide channels. An iterative electron beam lithography process provides a viable meth…
Fabrication and characterization of shape- and topology-optimized optical cavities with deep sub-wavelength confinement for interfacing with colloidal quantum dots
We report on a temporal evolution of photoluminescence (PL) spectroscopy of CuInS$_{2}$/ZnS colloidal quantum dots (QDs) by drop-casting on SiO$_{2}$/Si substrates and high quality factor microdisks (MDs) under different atmospheric conditions. Fast PL decay, peak blueshift and linewidth broadening due to photooxidation have been observed at low excitation power. With further increasing of the excitation power, the PL peak position shows a redshift and linewidth becomes narrow, which is ascribed to the enhanced F$\ddot{o}$rster resonant energy transfer between different QDs by photoinduced agg…
Colloidal quantum dots are robust, efficient, and tunable emitters now used in lighting, displays, and lasers. Consequently, when the spaser, a laser-like source of surface plasmons, was first proposed, quantum dots were specified as the ideal plasmonic gain medium. Subsequent spaser designs, however, have required a single material to simultaneously provide gain and define the plasmonic cavity, an approach ill-suited to quantum dots and other colloidal nanomaterials. Here we develop a more open architecture that decouples the gain medium from the cavity, leading to a versatile class of quantu…
Multiply-excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room temperature single-particle spectroscopy of their emission has so far proved elusive due to the temporal and spectral overlap with emission from the singly-excited and charged states. Here we introduce biexciton heralded spectroscopy, enabled by a single-photon avalanche diode array based spectrometer. This allows us to directly observe biexciton-exciton emission cascades an…
Engineering an array of precisely located cavity-coupled active media poses a major experimental challenge in the field of hybrid integrated photonics. We deterministically position solution processed colloidal quantum dots (QDs) on high quality-factor silicon nitride nanobeam cavities and demonstrate light-matter coupling. By lithographically defining a window on top of an encapsulated cavity that is cladded in a polymer resist, and spin coating QD solution, we can precisely control the placement of the QDs, which subsequently couple to the cavity. We show that the number of QDs coupled to th…
Systems of photonic crystal cavities coupled to quantum dots are a promising architecture for quantum networking and quantum simulators. The ability to independently tune the frequencies of laterally separated quantum dots is a crucial component of such a scheme. Here, we demonstrate independent tuning of laterally separated quantum dots in photonic crystal cavities coupled by in-plane waveguides by implanting lines of protons which serve to electrically isolate different sections of a diode structure.
We demonstrate a fiber in-line single photon source based on a hybrid system of colloidal single quantum dots deposited on an optical nanofiber and cooled down to cryogenic temperature (3.7 K). We show that a charged state (trion) of the single quantum dot exhibits a photo-stable emission of single photons with high quantum efficiency, narrow linewidth (3 meV FWHM) and fast decay time ($10.0\pm0.5$ ns). The single photons are efficiently coupled to the guided modes of the nanofiber and eventually to a single mode optical fiber. The brightness (efficiency) of the single photon source is estimat…
Materials with optical gain in the infrared are of paramount importance for optical communications, medical diagnostics and silicon photonics. The current technology is based either on costly III-V semiconductors that are not monolithic to silicon CMOS technology or Er-doped fiber technology that does not make use of the full fiber transparency window. Colloidal quantum dots (CQD) offer a unique opportunity as an optical gain medium in view of their tunable bandgap, solution processability and CMOS compatibility. The 8-fold degeneracy of infrared CQDs based on Pb-chalcogenides has hindered the…
Nanoantenna enhanced ultrafast emission from colloidal quantum dots as quantum emitters is required for fast quantum communications. On chip integration of such devices require a scalable and high throughput technology. We report self-assembly lithography technique of preparing hybrid of gold-nanorods antenna over a com- pact CdSe quantum dot monolayer. We demonstrate resonant and off resonant gold nanorod antenna enhanced radiative and anisotropic decay. Extensive simulations explain the mechanism of the decay rates and the role of antenna in both random and a compact monolayer of quantum dot…
In-Situ Quantum Optical Measurement for Colloidal Quantum Dots Confined in an Optical Trap
State Key Laboratory of Silicon and Advanced Semiconductor Materials（硅与先进半导体材料国家重点实验室）；College of Information Science and Electronic Engineering, Zhejiang University（浙江大学信息与电子工程学院）；Department of Chemistry, Zhejiang University（浙江大学化学系）；ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University（浙江大学杭州全球科创中心）；College of Optical Science and Engineering, Zhejiang University（浙江大学光电科学与工程学院）
Unique optical properties of colloidal semiconductor quantum dots (QDs), arising from quantum mechanical confinement of charge within these structures, present a versatile testbed for the study of how high electric fields affect the electronic structure of nanostructured solids. Earlier studies of quasi-DC electric field modulation of QD properties have been limited by the electrostatic breakdown processes under the high externally applied electric fields, which have restricted the range of modulation of QD properties. In contrast, in the present work we drive CdSe:CdS core:shell QD films with…
Room-temperature cavity exciton-polariton condensation in perovskite quantum dots
IBM Research Europe – Zurich（IBM欧洲苏黎世研究中心）；ETH Zurich（苏黎世联邦理工学院）；Institute of Materials Science of Sevilla, Consejo Superior de Investigaciones Científicas − Universidad de Sevilla (CSIC-US)（塞维利亚材料科学研究所，西班牙国家研究委员会-塞维利亚大学）；Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich（苏黎世联邦理工学院化学与应用生物科学学院无机化学实验室）；Empa − Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科学与技术研究院）
We have studied the variation in fine-structure splitting (FSS) under application of vertical electric field in a range of quantum dots grown by different methods. In each sample we confirm that this energy splitting changes linearly over the field range we can access. We conclude that this linear tuning is a general feature of self-assembled quantum dots, observed under different growth conditions, emission wavelengths and in different material systems. Statistical measurements of characteristic parameters such as emission energy, Stark shift and FSS tuning are presented which may provide a g…
Images of semiconductor `dot in rods' and their small clusters are studied by measuring the second-order correlation function with a spatially resolving ICCD camera. This measurement allows one to distinguish between a single dot and a cluster and, to a certain extent, to estimate the number of dots in a cluster. A more advanced measurement is proposed, based on higher-order correlations, enabling more accurate determination of the number of dots in a small cluster. Nonclassical features of the light emitted by such a cluster are analyzed.
We use an optical fiber taper waveguide to probe PbS quantum dots (QDs) dried on Si photonic crystal cavities near 1.55 $μ$m. We demonstrate that a low density ($\lesssim 100 μ$m$^{-2}$) of QDs does not significantly degrade cavity quality factors as high as $\approx3\times10^4$. We also show that the tapered fiber can be used to excite the QDs and collect the subsequent cavity-filtered photoluminescence, and present measurements of reversible photodarkening and QD saturation. This method represents an important step towards spectroscopy of single colloidal QDs in the telecommunications band.
In this work we develop a simple theory for the green photoluminescence of ZnO quantum dots (QDs) that allows us to understand and rationalize several experimental findings on fundamental grounds. We calculate the spectrum of light emitted in the radiative recombination of a conduction band electron with a deeply trapped hole and find that the experimental behavior of this emission band with particle size can be understood in terms of quantum size effects of the electronic states and their overlap with the deep hole.We focus the comparison of our results on detailed experiments performed for c…
Individual colloidal quantum dots can be optically trapped and manipulated by a single infrared laser beam operated at low laser powers. If the absorption spectrum and the emission wavelength of the trapping laser are appropriately chosen, the trapping laser light can act as a source for two-photon excitation of the trapped quantum dot. This eliminates the need for an additional excitation laser in experiments where individual quantum dots are used both as force transducers and for visualization of the system. To use quantum dots as handles for quantitative optical force transduction, it is cr…
We demonstrate an important step towards on chip integration of single photon sources operating at room temperature fiber coupling of a directional quantum emitter with back-excitation. Directionality is achieved with a hybrid metal-dielectric bullseye antenna, while back-excitation is permitted by placement of the emitter at or in a sub-wavelength hole positioned at the bullseye center. Overall, the unique design enables a direct laser excitation from the back of the on-chip device and very efficient coupling of the highly collimated photon emission to either low numerical aperture (NA) free …
Optical and X-ray Photo-emission Spectroscopies of Core/Shell Colloidal CdSe/CdS Quantum Dots: Modeling and Experimental Determination of Band Alignment
In this work, we report the first account of monolithically-fabricated vertical cavity surface emitting lasers (VCSELs) of densely-packed, orientation-controlled, atomically flat colloidal quantum wells (CQWs) using a self-assembly method and demonstrate single-mode lasing from a record thin colloidal gain medium with a film thickness of 7 nm under femtosecond optical excitation. We used specially engineered CQWs to demonstrate these hybrid CQW-VCSELs consisting of only a few layers to a single monolayer of CQWs and achieved the lasing from these thin gain media by thoroughly modeling and impl…
The excitonic fine structure plays a key role for the quantum light generated by semiconductor quantum dots, both for entangled photon pairs and single photons. Controlling the excitonic fine structure has been demonstrated using electric, magnetic, or strain fields, but not for quantum dots in optical cavities, a key requirement to obtain high source efficiency and near-unity photon indistinguishability. Here, we demonstrate the control of the fine structure splitting for quantum dots embedded in micropillar cavities. We propose a scheme based on remote electrical contacts connected to the pi…
The scalability of quantum dot based non-classical light sources relies on the control over their dissimilar emission energies. Electric fields offer a promising route to tune the quantum dot emission energy through the quantum-confined Stark effect. However, electric fields have been mostly used for tuning the energy of single-photon emission from quantum dots, while electrical control over the energy of entangled-photon emission, which is crucial for building a solid-state quantum repeater using indistinguishable entangled photons, has not been realized yet. Here, we present a method to achi…
A high-Q Split Cavity Enabling Independent Electrical Tuning of two Quantum Dots
University of Delaware（特拉华大学）；Quantum Science and Engineering Program, University of Delaware（特拉华大学量子科学与工程计划）；Department of Materials Science and Engineering, University of Delaware（特拉华大学材料科学与工程系）
We investigate the fluorescence properties of colloidal quantum dots attached to gold rod nanoantennas. These structures are fabricated by a two step electron beam lithography process in combination with a chemical linking method. By varying the nanoantenna length, the plasmon modes of the nanoantennas are successively tuned through the emission band of the quantum dots. We observe a pronounced fluorescence enhancement both for short and long nanoantennas. These findings can be attributed to the coupling of the quantum dots to bright and dark plasmon modes, respectively.
We report the broadband (~ 25 nm) enhancement of radiative decay rate of colloidal quantum dots by exploiting the hyperbolic dispersion of a one-dimensional nonmagnetic metamaterial structure.
Two-photon excitation in the near-infrared (NIR) of colloidal nanocrystalline silicon quantum dots (nc-SiQDs) with photoluminescence also in the NIR has the potential to open up new opportunities in the field of deep biological imaging. Spectra of the degenerate two-photon absorption (2PA) cross section of colloidal nc-SiQDs are measured using two-photon excitation over a spectral range $1.46 < \hbar ω< 1.91$ eV (wavelength $850 > λ> 650$ nm) above the two-photon band gap $E_g^{(QD)}/2$, and at a representative photon energy $\hbar ω= 0.99$ eV ($λ= 1250$ nm) below this gap. Two-photon excited …
